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We report a Raman scattering study of six rare earth orthoferrites RFeO3,with R = La, Sm, Eu, Gd, Tb, Dy. The use of extensive polarized Ramanscattering of SmFeO3 and first-principles calculations enable the assignment ofthe observed phonon modes to vibrational symmetries and atomic displacements.The assignment of the spectra and their comparison throughout the whole seriesallows correlating the phonon modes with the orthorhombic structuraldistortions of RFeO3 perovskites. In particular, the positions of two specificAg modes scale linearly with the two FeO6 octahedra tilt angles, allowing thedistortion throughout the series. At variance with literature, we find that thetwo octahedra tilt angles scale differently with the vibration frequencies oftheir respective Ag modes. This behavior as well as the general relationsbetween the tilt angles, the frequencies of the associated modes and the ionicradii are rationalized in a simple Landau model. The reported Raman spectra andassociated phonon-mode assignment provide reference data for structuralinvestigations of the whole series of orthoferrites.

Raman spectroscopy of rare-earth orthoferrites RFeO3 (R = La, Sm, Eu, Gd, Tb, Dy)